Tunable Mesoscale Chirality in Two-Dimensional Vortex-like Assemblies of Helically Grooved Poly(phenylacetylene) Derivatives

Two-dimensional (2D) chiral materials offer exciting opportunities in sensing and catalysis, yet achieving mesoscale chirality in 2D organic assemblies remains challenging. We introduce a bioinspired strategy to fabricate 2D vortex-like platelets with mesoscale chirality from DNA-mimicking helically grooved poly(phenylacetylene) derivatives via interchain twisted coupling. By tuning assembly kinetics including solvent exchange rate and temperature, we program both the handedness and curvature of mesoscopic chirality. Theoretical simulations show that inherent chain helicity dictates twist direction, while assembly conditions govern angular magnitude. Polymers with helical grooves outperform rigid rod-like analogues: their fluted surfaces serve as stereochemical "hotspots", channeling torsional stress to enable directional coupling across the plane. Dependence of mesoscale chirality on polymer molecular weights further confirms the universality of helical-groove-driven chiral amplification. These vortex platelets exhibit enhanced circularly polarized luminescence (CPL) superior to regular achiral 2D ones. This work offers new insights into both mechanistic understanding of hierarchical chirality transfer and an engineering framework for biomimetic mesoscale chiral materials.